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This study presents a twofold methodological approach to investigate the physicochemical behaviour of IGI\u2010based formulations found in historical Portuguese sources. Fresh and 6\u2010month naturally aged precipitates and supernatant solutions (dried inks) were characterised, and the impact of IGIs on Whatman paper over ageing was studied using attenuated total reflectance Fourier\u2010transform infrared (ATR\u2010FT\u2010IR) spectroscopy, Raman and M\u00f6ssbauer spectroscopies and X\u2010ray diffraction (XRD). Iron(II) sulphates comprised the primary crystalline phase in the precipitates, while the dried inks consisted of distinct Fe(III)\u2010polyphenol (PPh) complexes. Over time, Fe(III) M\u00f6ssbauer parameters supported complex structural alterations. IGI\u2010induced degradation on aged mockups was attested by Fe(II) oxalate formation until total depletion of the Fe(III)\u2010PPh fraction. pH, ATR\u2010FT\u2010IR and degree of polymerisation analyses suggested that cellulose oxidation is the primary degradation mechanism, and the physical properties and XRD corroborated that the cellulose structure became disordered over ageing. The ink with the higher weight ratio of Fe(II) sulphate:gallnuts (unbalanced) exhibited the most aggressive action on the support. The results confirm that the more unbalanced the ink composition, the more severe its impact, with ink concentration per surface area also being a critical factor in paper decay.<\/jats:p>","DOI":"10.1002\/cplu.202500369","type":"journal-article","created":{"date-parts":[[2026,1,30]],"date-time":"2026-01-30T10:40:07Z","timestamp":1769769607000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["From Ink to Mockup: An Integrated Study of Historical Gall Ink Formulations and Their Impact on Paper"],"prefix":"10.1002","volume":"91","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-3286-5135","authenticated-orcid":false,"given":"Margarida","family":"Nunes","sequence":"first","affiliation":[{"name":"Universidade de \u00c9vora, HERCULES Laboratory\/IN2PAST  \u00c9vora Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6098-9581","authenticated-orcid":false,"given":"Joana Costa","family":"Vieira","sequence":"additional","affiliation":[{"name":"FibEnTech\u2010UBI Fiber Materials and Environmental Technologies University of Beira Interior  Covilh\u00e3 Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1583-3462","authenticated-orcid":false,"given":"Ana Paula","family":"Costa","sequence":"additional","affiliation":[{"name":"FibEnTech\u2010UBI Fiber Materials and Environmental Technologies University of Beira Interior  Covilh\u00e3 Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9686-1312","authenticated-orcid":false,"given":"Maria Em\u00edlia Amaral","family":"Cabral","sequence":"additional","affiliation":[{"name":"FibEnTech\u2010UBI Fiber Materials and Environmental Technologies University of Beira Interior  Covilh\u00e3 Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6536-9875","authenticated-orcid":false,"given":"Bruno J. 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